US11380909B2 - Method of manufacturing separator - Google Patents

Method of manufacturing separator Download PDF

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Publication number
US11380909B2
US11380909B2 US17/128,547 US202017128547A US11380909B2 US 11380909 B2 US11380909 B2 US 11380909B2 US 202017128547 A US202017128547 A US 202017128547A US 11380909 B2 US11380909 B2 US 11380909B2
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Prior art keywords
bead
separator
stopper
preload
seal section
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US17/128,547
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US20210194019A1 (en
Inventor
Yohei Sano
Shigeru Watanabe
Akihito GIGA
Suguru OHMORI
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Honda Motor Co Ltd
Nok Corp
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Honda Motor Co Ltd
Nok Corp
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Assigned to HONDA MOTOR CO., LTD., NOK CORPORATION reassignment HONDA MOTOR CO., LTD. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: Ohmori, Suguru, GIGA, AKIHITO, SANO, YOHEI, WATANABE, SHIGERU
Publication of US20210194019A1 publication Critical patent/US20210194019A1/en
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0206—Metals or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0273—Sealing or supporting means around electrodes, matrices or membranes with sealing or supporting means in the form of a frame
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0223—Composites
    • H01M8/0228—Composites in the form of layered or coated products
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0276—Sealing means characterised by their form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286—Processes for forming seals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a method of manufacturing a separator for use in a fuel cell.
  • FIG. 7 is a cross-sectional view illustrating a separator according to the related art.
  • a separator 120 includes a first metal separator 101 , a second metal separator 102 , and seal members 113 and 113 .
  • Each of the first metal separator 101 and the second metal separator 102 includes a protruding sealing bead portion 111 and protruding stopper bead portions 112 having a protruding height lower than that of the sealing bead portion 111 .
  • a bead seal section 121 is formed of the sealing bead portions 111 and 111 and the seal members 113 and 113 .
  • each stopper section 122 is formed of the stopper bead portions 112 and 112 .
  • the bead seal sections 121 and 121 facing each other hold and seal an electrolyte membrane in between, and thereby are capable of preventing leakage of reaction gas such as fuel gas and oxidant gas. Further, when an excessive pressing load acts on a fuel cell, the stopper sections 122 receive the load and make the bead seal section 121 less likely to be excessively distorted or bucked.
  • FIG. 8 is a schematic diagram illustrating a preload applying step in a separator according to the related art.
  • the preload can be applied to the separator 120 by a pair of plate-shaped platens 140 and 140 . If the bead seal section 121 is deformed in advance by the load acting in directions reverse to the protruding directions of the sealing bead portions 111 , the bead seal section 121 can achieve stable sealing performance without inducing plastic deformation even when the pressing load acting on the bead seal section 121 varies.
  • FIG. 9 is a graph presenting a relationship between a deformation amount and a pressing load of a bead seal section and stopper sections in a separator according to the related art.
  • a pressing load is applied along a load characteristic line L 1 to the bead seal section 121 (point a) that has not been deformed in advance
  • the bead seal section 121 exhibits the sealing performance (point b).
  • point c when a pressing load due to a disturbance acts (point c), the bead seal section 121 is plastically deformed and the load characteristic line of the bead seal section 121 moves from L 1 to L 2 . For this reason, the bead seal section 121 has difficulty in maintaining the stable sealing performance.
  • FIG. 10 is a graph presenting a relationship between a pressing load and a linear pressure occurring in a bead seal section in a separator according to the related art.
  • the bead seal section 121 may fail to generate a required linear pressure because the stopper sections 122 receive a part of the pressing load (see a region W 1 ).
  • the bead seal section 121 may be abnormally deformed and impair the sealing function (see region W 2 ). For these reasons, the high dimensional accuracy is required for the height of the stopper sections 122 (the stopper bead portions 112 ).
  • the present invention has been made to solve the aforementioned problem, and has an object to provide a method of manufacturing a separator capable of achieving a desired sealing surface pressure without inducing plastic deformation even with a load variation.
  • the present invention for solving the aforementioned problem provides a method of manufacturing a separator for use in a fuel cell, the method including a forming step of forming a first metal separator and a second metal separator each including a protruding sealing bead portion and a protruding stopper bead portion having a protruding height lower than that of the sealing bead portion; a joining step of joining surfaces of the first metal separator and the second metal separator on sides opposite to sides on which their respective sealing bead portions protrude, and attaching seal members in an extension direction or on distal ends of the sealing bead portion; and a preload applying step of applying preload to a bead seal section formed of one pair of the sealing bead portions and the seal members and a stopper section formed of one pair of the stopper bead portions in a height direction thereof, thereby plastically deforming the bead seal section and the stopper section simultaneously.
  • a dimensional variation of the height of the stopper bead portions can be reduced because the preload is applied to the stopper section. This makes it possible to achieve a desired sealing surface pressure even in the case where a load variation occurs in a fuel cell.
  • the preload is applied to both of the sealing bead portions and the stopper bead portions, it is possible to achieve a desired sealing surface pressure without inducing plastic deformation even with a load variation.
  • FIG. 1 is a cross-sectional view of a fuel cell according to Example 1.
  • FIG. 2 is a cross-sectional view illustrating a press forming step in a method of manufacturing a separator according to Example 1.
  • FIG. 3 is a cross-sectional view illustrating a state before load application in a preload applying step in the method of manufacturing a separator according to Example 1.
  • FIG. 4 is a cross-sectional view illustrating a state during load application in the preload applying step in the method of manufacturing a separator according to Example 1.
  • FIG. 5 is a graph presenting a relationship between a predeformation amount and a height of stopper sections in Example 1.
  • FIG. 6 is a cross-sectional view illustrating a preload applying step in a method of manufacturing a separator according to Example 2.
  • FIG. 7 is a cross-sectional view illustrating a separator according to the related art.
  • FIG. 8 is a schematic cross-sectional view illustrating a preload applying step in a separator according to the related art.
  • FIG. 9 is a graph presenting a relationship between a deformation amount and a pressing load of a bead seal section and stopper sections in a separator according to the related art.
  • FIG. 10 is a graph presenting a relationship between a pressing load and a linear pressure occurring in a bead seal section in a separator according to the related art.
  • a fuel cell 1 includes a membrane electrode assembly 2 , and a first separator 3 and a second separator 4 between which the membrane electrode assembly 2 is held.
  • Each of the first separator 3 and the second separator 4 is a separator assembly including a first metal separator 21 , a second metal separator 22 , and seal members 51 and 51 .
  • Each of the first metal separator 21 and the second metal separator 22 includes a protruding sealing bead portion 31 and protruding stopper bead portions 32 having a protruding height lower than that of the sealing bead portion 31 .
  • the sealing bead portions 31 and 31 and the seal members 51 and 51 form the bead seal section 41 .
  • the stopper bead portions 32 and 32 form the stopper sections 42 .
  • preload is applied to both of the bead seal section 41 and the stopper sections 42 . This makes it possible to achieve a desired sealing surface pressure without inducing plastic deformation even with a load variation.
  • the fuel cell 1 is a member that generates power through chemical reaction between hydrogen (fuel gas) supplied from an anode side and oxygen (oxidant gas) supplied from a cathode side.
  • a fuel cell stack is formed by stacking multiple fuel cells 1 and applying a predetermined compressing load to the fuel cells 1 in a stacking direction thereof.
  • FIG. 1 illustrates the fuel cell 1 under the condition where a predetermined compressing load is applied.
  • the membrane electrode assembly (MEA) 2 includes an electrolyte membrane 11 , electrode catalyst layers 12 and 12 , and gas diffusion layers 13 and 13 .
  • the electrolyte membrane 11 spreads outside the gas diffusion layers 13 .
  • a portion of the electrolyte membrane 11 spreading outside the gas diffusion layers 13 may be a resin film (resin flame member) in some cases.
  • the first separator 3 is a plate-shaped member arranged on one side of the membrane electrode assembly 2 (on the lower side in FIG. 1 ).
  • the second separator 4 is a plate-shaped member arranged on the other side of the membrane electrode assembly 2 (on the upper side in FIG. 1 ). Since the first separator 3 and the second separator 4 in the present example have the same structure, the detailed description of the second separator 4 is omitted with the same reference signs as in the first separator 3 assigned to the second separator 4 .
  • the first separator 3 includes a bead seal section 41 forming a seal region R 1 and stopper sections 42 .
  • the stopper sections 42 are sections that, when a disturbance (such as a temperature change or collision) occurs on a stack, give support to prevent the bead seal section 41 from being deformed excessively beyond a preset maximum compression amount (receive the load due to the disturbance).
  • the bead seal section 41 protrudes toward the electrolyte membrane 11 (or the resin film) and is formed, for example, in an endless form along the entire outer periphery of the fuel cell 1 .
  • only one bead seal section 41 is provided, but two or more bead seal sections 41 may be provided.
  • the bead seal section 41 is provided with the seal members 51 in its extension direction or on the distal ends along the extension direction.
  • the seal member 51 is formed of an elastic material and is a flat gasket having a rectangular cross section in the present example.
  • the seal member 51 is formed by applying a liquid resin material.
  • the thickness of the seal member 51 may be set as appropriate, but may be set to, for example, about 50 to 200 ⁇ m.
  • the seal member 51 may be formed of a material having elasticity. For example, ethylene propylene diene rubber (EPDM), silicone rubber (VMQ), fluororubber (FKM), polyisobutylene (PIB), SIFEL (registered trademark: Shin-Etsu Chemical Co., Ltd.), a resin or the like may be used.
  • Each of the stopper sections 42 protrudes toward the electrolyte membrane 11 and contacts with the electrolyte membrane 11 or faces the electrolyte membrane 11 across a slight space.
  • the stopper section 42 is extended in a linear form or curved form along the extension direction of the bead seal section 41 .
  • the seal region R 1 is formed in such a way that the bead seal section 41 of the first separator 3 and the bead seal section 41 of the second separator 4 hold the electrolyte membrane 11 in between.
  • the seal region R 1 makes it possible to prevent leakage of reaction gas such as fuel gas and oxidant gas. Since both the facing bead seal sections 41 include the seal members 51 , the sealing performance can be enhanced.
  • reaction surfaces or channel portions 43 form reaction surfaces or channel portions 43 .
  • the reaction surfaces or channel portions 43 in the first separator 3 and the reaction surfaces or channel portions 43 in the second separator 4 hold the membrane electrode assembly 2 (the gas diffusion layers 13 and 13 ) in between, thereby forming a reaction region through which the reaction gas flows.
  • Preload is applied to all of the bead seal sections 41 and the stopper sections 42 in the first separator 3 and the second separator 4 .
  • the preload will be described later.
  • the method of manufacturing a separator in the present example includes a press forming step (forming step), a bonding step, and a preload applying step.
  • the press forming step is a step of press-forming the first metal separator 21 and the second metal separator 22 as illustrated in FIG. 2 .
  • a flat metal thin plate (material) having a thickness of about 0.03 to 0.5 mm is press-formed to have a corrugated cross section, thereby forming the first metal separator 21 and the second metal separator 22 .
  • the first metal separator 21 includes a sealing bead portion 31 and stopper bead portions 32 (two stopper bead portions 32 on each side of the sealing bead portion 31 in the present example).
  • the sealing bead portion 31 and the stopper bead portions 32 each have a full bead shape having a protruding cross-sectional shape.
  • the protruding height of the stopper bead portions 32 in the plate-thickness direction is lower than that of the sealing bead portion 31 .
  • the numbers and layout of the sealing bead portion 31 and the stopper bead portions 32 are just an example, and may be set as appropriate.
  • the joining step is a step of joining the first metal separator 21 and the second metal separator 22 together and attaching the seal members 51 .
  • the surfaces of the first metal separator 21 and the second metal separator 22 on the sides opposite to the sides on which their respective sealing bead portions 31 protrude are joined together.
  • the first metal separator 21 and the second metal separator 22 are united by brazing, swaging, welding, or the like.
  • the seal members 51 and 51 are attached in the extension direction or to the distal ends of the sealing bead portions 31 and 31 .
  • the bead seal section 41 is formed of the sealing bead portions 31 and 31 and the seal members 51 and 51 .
  • a hollow cavity is formed in the bead seal section 41 .
  • the stopper section 42 is formed of the stopper bead portions 32 and 32 .
  • a hollow cavity is formed in the stopper section 42 .
  • the preload applying step is a step of applying preload to the first metal separator 21 , the second metal separator 22 , and the seal members 51 united in the joining step (hereinafter also referred to as the “pressed-joined body”) by using platens 61 and 61 as illustrate in FIGS. 3 and 4 .
  • the platens 61 are members that apply the preload to the pressed-joined body.
  • the platens 61 are arranged in pair on both sides of the pressed-joined body.
  • Each of the platens 61 is formed of a high-strength metal or resin and has a plate-like shape.
  • the platen 61 includes a pressing surface 62 and a recessed groove portion 63 .
  • the pressing surface 62 is a flat surface facing the stopper sections 42 in the pressed-joined body.
  • the recessed groove portion 63 is a groove provided at a center portion of the pressing surface 62 and having a rectangular cross section.
  • the depth of the recessed groove portion 63 is set as appropriate based on the magnitudes of preload to be applied to the bead seal section 41 and the stopper sections 42 . In other words, the magnitudes of the preload to be applied to the bead seal section 41 and the stopper sections 42 can be controlled by adjusting the depth of the recessed groove portion 63 .
  • the width of the recessed groove portion 63 is set to such a width that the recessed groove portion 63 and the sealing bead portion 31 may not interfere with each other in an operation of applying the preload.
  • the platens 61 and 61 are brought close to each other from both sides of the pressed-joined body while the bead seal section 41 is placed inside the recessed groove portions 63 of the platens 61 .
  • the load is simultaneously applied to both of the bead seal section 41 and the stopper sections 42 from the platens 61 and 61 .
  • the magnitudes of the preload may be set as appropriate, but may be set to, for example, a greatest load that may act on a fuel cell stack in the stack direction during power generation.
  • the platens 61 are pulled apart from the pressed-joined body to release the load.
  • each of the first separator 3 and the second separator 4 is formed.
  • the method of manufacturing a separator is not limited to the above steps. For example, the order of the steps and the materials may be modified as appropriate.
  • the assembling step is a step of holding the membrane electrode assembly 2 (the electrolyte membrane 11 ) between the first separator 3 and the second separator 4 as illustrated in FIG. 1 .
  • the compressing step is a step of forming a fuel cell stack by stacking multiple fuel cells assembled and applying a predetermined compressing load to the fuel cells as illustrated in FIG. 1 .
  • the seal region R 1 is formed.
  • the stopper sections 42 and the electrolyte membrane 11 contact with each other or face each other across a slight space.
  • FIG. 5 is a graph presenting a relationship between a predeformation amount and the height of the stopper sections in Example 1.
  • a region between two solid lines indicates a dimensional variation range of the stopper sections 42 .
  • the height variation of the stopper sections 42 is large. Separators formed under the above condition may not achieve the desired sealing performance if a load variation occurs as described above.
  • the height variation of the stopper sections 42 was reduced in the case where the predeformation amount was in a range of YT 1 to YT 2 , as presented in FIG. 5 .
  • the dimensional accuracy of the stopper sections 42 can be enhanced, so that it is possible to prevent a deterioration of the sealing function due to a dimensional variation of the stopper sections 42 .
  • the stopper sections 42 and 42 facing each other can give support to prevent the bead seal section 41 from being deformed excessively beyond a preset maximum compression amount. This enables the bead seal section 41 to offer a stable linear pressure and thereby achieve a desired sealing surface pressure stably.
  • the preload can be easily applied to both of the bead seal section 41 and the stopper sections 42 .
  • the load to act on the stopper sections 42 can be easily controlled irrespective of the preload to be applied to the bead seal section 41 .
  • the load to act on each of the bead seal section 41 and the stopper sections 42 (the predeformation amount) can be changed by adjusting the depth of the recessed groove portion 63 .
  • a portion for the recessed groove portion 63 is formed in a nested structure, and the depth of the recessed groove portion 63 is adjusted by inserting a shim between the mother die for the platen 61 and the nested portion.
  • multiple platens 61 including recessed groove portions 63 having different depths may be prepared and be exchanged as appropriate for the adjustment.
  • the preload can be simultaneously applied to both of the bead seal section 41 and the stopper sections 42 , and therefore steps (differences in height dimension) between the bead seal section 41 and the stopper sections 42 can be equalized.
  • the bead seal section 41 is on a load characteristic line before plastic deformation when no load is applied, but moves to a load characteristic line different from the load characteristic line before plastic deformation when a load is applied. This narrows an operation range for maintaining the desired sealing surface pressure and makes it difficult to obtain a wide operation range in which the separator can withstand a disturbance (such as a temperature change or collision).
  • both of the bead seal section 41 and the stopper sections 42 are plastically deformed in advance.
  • the bead seal section 41 and the stopper sections 42 are not plastically deformed due to a load variation during operation of a fuel cell stack, and can move on the same load characteristic line in both cases with load application and load removal. Accordingly, it is possible to widen the operation range, obtain wide load characteristics in which the separator can withstand a disturbance (such as a temperature change or collision), and therefore surely achieve a desired sealing surface pressure.
  • the preload is applied to both of the bead seal sections 41 (the sealing bead portions 31 and the seal members 51 ) and the stopper sections 42 (the stopper bead portions 32 ) of the first separator 3 and the second separator 4 , so that the sealing performance can be synergistically improved without inducing plastic deformation even with a variation of the pressing load.
  • Example 2 is different from Example 1 in that platens 61 A and spacers 71 are used.
  • the platens 61 A and four spacers 71 are prepared.
  • the pressing surface 62 of each of the platens 61 A is flat (having no recessed groove portion).
  • the spacers 71 and 71 are fixed to the platen 61 A and one spacer 71 is arranged on each of both sides of a center portion of the platen 61 A.
  • the seal members 51 and 51 of the bead seal section 41 are placed in contact with the pressing surfaces 62 and 62 and both ends of the stopper sections 42 are placed in contact with the spacers 71 and 71 .
  • the platens 61 A and 61 A are brought close to each other to apply the preload to the bead seal section 41 and the stopper sections 42 .
  • Example 2 described above can also produce substantially the same effects as in Example 1.
  • the load to act on the bead seal section 41 and the stopper sections 42 can be easily controlled by adjusting the thickness dimension of the spacers 71 .
  • stopper sections 42 are arranged on both sides of the electrolyte membrane 11 , but may be arranged on only one of the sides.

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  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Composite Materials (AREA)
  • Fuel Cell (AREA)
US17/128,547 2019-12-23 2020-12-21 Method of manufacturing separator Active US11380909B2 (en)

Applications Claiming Priority (3)

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JP2019-231111 2019-12-23
JP2019231111A JP7264802B2 (ja) 2019-12-23 2019-12-23 セパレータの製造方法
JPJP2019-231111 2019-12-23

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US20210194019A1 US20210194019A1 (en) 2021-06-24
US11380909B2 true US11380909B2 (en) 2022-07-05

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JP7344802B2 (ja) * 2020-01-27 2023-09-14 Nok株式会社 燃料電池のシール構造
JP7436350B2 (ja) * 2020-11-27 2024-02-21 Nok株式会社 セパレータの製造方法
DE202022104298U1 (de) 2022-07-28 2023-11-02 Reinz-Dichtungs-Gmbh Dichtlage, Separatorplatte und Elektrolyseur

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